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Effect of CO2 on the selective catalytic reduction of NOx with NH3 of Fe0.4Ce0.6O2-δ catalyst: adsorption behavior
Surfaces and Interfaces ( IF 5.7 ) Pub Date : 2021-04-01 , DOI: 10.1016/j.surfin.2021.101118
Hui Wang , Shicheng Dong , Yujie Qiao , Zhenping Qu

Besides of NOx, CO2 is always abundantly present in the exhaust gas stream, which is important for the investigation of de-NOx. The presence of CO2 has an inhibiting effect on the NH3-SCR activity at temperatures below 300°C for the Fe0.4Ce0.6O2-δ catalysts. To make clear this impact of CO2 for NH3-SCR reaction, we further investigate the changes of NH3 and NOx adsorption behaviors, using in situ TPD and in situ DRIFTS technologies. The DRIFT spectra of CO2 adsorption show that weakly adsorbed carbonate and bicarbonate species were formed, leading to the changes in adsorption and activation behaviors of NH3 and NOx. On the one hand, the formed carbonate and bicarbonate can act as new acid sites thereby improvement of NH3 adsorption. On the other hand, the adsorption of NOx on Fe-O-Ce is suppressed by CO2 results from its competitive adsorption. Especially, the formation path of monodentate nitrate may be blocked by CO2, which is usually active intermediate species for the NH3-SCR reaction, resulting in the deactivation of CO2.



中文翻译:

CO 2对Fe 0.4 Ce 0.6 O2 催化剂的NH 3选择性催化还原NH x的影响:吸附行为

除了NO x之外,废气流中始终富含CO 2,这对于研究de-NO x至关重要。对于Fe 0.4 Ce 0.6 O2 催化剂,在低于300°C的温度下,CO 2的存在对NH 3 -SCR活性具有抑制作用。为了弄清楚CO 2对NH 3 -SCR反应的影响,我们使用原位TPD和原位DRIFTS技术进一步研究了NH 3和NO x吸附行为的变化。CO 2的DRIFT光谱吸附表明形成了弱吸附的碳酸盐和碳酸氢盐物质,导致NH 3和NO x的吸附和活化行为发生了变化。一方面,形成的碳酸盐和碳酸氢盐可以充当新的酸位,从而改善了NH 3的吸附。另一方面,由于竞争性吸附而产生的CO 2抑制了NO x在Fe-O-Ce上的吸附。特别地,单齿硝酸盐的形成路径可能被CO 2阻塞,而CO 2通常是NH 3 -SCR反应的活性中间物种,导致CO 2失活。

更新日期:2021-04-13
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